High-order-harmonic generation in homonuclear and heteronuclear diatomic molecules: Exploration of multiple orbital contributions

We present a time-dependent density functional theory (TDDFT) approach with proper asymptotic long-range potential for nonperturbative treatment of high-order harmonic generation (HHG) of diatomic molecules with their molecular axis parallel to the laser field polarization. A time-dependent two-cent...

Full description

Saved in:
Bibliographic Details
Published in:Physical review. A, Atomic, molecular, and optical physics Atomic, molecular, and optical physics, 2011-04, Vol.83 (4), Article 043414
Main Authors: Heslar, John, Telnov, Dmitry, Chu, Shih-I
Format: Article
Language:English
Subjects:
ASYMPTOTIC SOLUTIONS
ATOMIC AND MOLECULAR PHYSICS
CALCULATION METHODS
CARBON COMPOUNDS
CARBON MONOXIDE
CARBON OXIDES
CHALCOGENIDES
CONFIGURATION
DENSITY FUNCTIONAL METHOD
ELECTROMAGNETIC RADIATION
ELECTRONS
ELEMENTARY PARTICLES
ELEMENTS
FERMIONS
FLUORINE
FLUORINE COMPOUNDS
FREQUENCY MIXING
HALOGEN COMPOUNDS
HALOGENS
HARMONIC GENERATION
HYDROFLUORIC ACID
HYDROGEN COMPOUNDS
INORGANIC ACIDS
INORGANIC COMPOUNDS
INTERFERENCE
LASER RADIATION
LEPTONS
MATHEMATICAL SOLUTIONS
MOLECULAR ORBITAL METHOD
MOLECULES
NITROGEN
NONLINEAR PROBLEMS
NONMETALS
OXIDES
OXYGEN COMPOUNDS
POLARIZATION
POTENTIALS
PULSES
RADIATIONS
SPACE DEPENDENCE
SPECTRA
SPHERICAL CONFIGURATION
TIME DEPENDENCE
VARIATIONAL METHODS
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:We present a time-dependent density functional theory (TDDFT) approach with proper asymptotic long-range potential for nonperturbative treatment of high-order harmonic generation (HHG) of diatomic molecules with their molecular axis parallel to the laser field polarization. A time-dependent two-center generalized pseudospectral method in prolate spheroidal coordinate system is used for accurate and efficient treatment of the TDDFT equations in space and time. The theory is applied to a detailed all-electron nonperturbative investigation of HHG processes of homonuclear (N{sub 2} and F{sub 2}) and heteronuclear (CO, BF, and HF) molecules in intense ultrashort laser pulses with the emphasis on the role of multiple molecular orbitals (MOs). The results reveal intriguing and substantially different nonlinear optical response behaviors for homonuclear and heteronuclear molecules. In particular, we found that the HHG spectrum for homonuclear molecules features a destructive interference of MO contributions while heteronuclear molecules show mostly constructive interference of orbital contributions.
ISSN:1050-2947
1094-1622
DOI:10.1103/PhysRevA.83.043414